Free tropospheric aerosols at the Mt. Bachelor Observatory: more oxidized and higher sulfate content compared to boundary layer aerosols

摘要

Understanding the properties and life cycle processes of aerosol particles in regional air masses is crucial for constraining the climate impacts of aerosols on a global scale. In this study, characteristics of aerosols in the boundary layer (BL) and free troposphere (FT) of a remote continental region in the western US were studied using a high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) deployed at the Mount Bachelor Observatory (MBO; 2763ma.s.l.) in central Oregon in summer 2013. In the absence of wildfire influence, the average (+/- 1 sigma) concentration of non-refractory submicrometer particulate matter (NR-PM1) at MBO was 2.8 (+/- 2.8) mu gm(-3) and 84% of the mass was organic. The other NR-PM1 components were sulfate (11 %), ammonium (2.8 %), and nitrate (0.9 %). The organic aerosol (OA) at MBO from these clean periods showed clear diurnal variations driven by the boundary layer dynamics with significantly higher concentrations occurring during daytime, upslope conditions. NR-PM1 contained a higher mass fraction of sulfate and was frequently acidic when MBO resided in the FT. In addition, OA in the FT was found to be highly oxidized (average O/C of 1.17) with low volatility while OA in BL-influenced air masses was moderately oxidized (average O/C of 0.67) and semivolatile. There are indications that the BL-influenced OA observed at MBO was more enriched in organonitrates and organosulfur compounds (e.g., MSA) and appeared to be representative of biogenic secondary organic aerosol (SOA) originated in the BL. A summary of the chemical compositions of NR-PM1 measured at a number of other high-altitude locations in the world is presented and similar contrasts between FT and BL aerosols were observed. The significant compositional and physical differences observed between FT and BL aerosols may have important implications for understanding the climate effects of regional background aerosols.